CN102820476A - Application of proton exchange membrane in Fe-Cr system liquid phase fluid battery - Google Patents

Application of proton exchange membrane in Fe-Cr system liquid phase fluid battery Download PDF

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CN102820476A
CN102820476A CN2011104490491A CN201110449049A CN102820476A CN 102820476 A CN102820476 A CN 102820476A CN 2011104490491 A CN2011104490491 A CN 2011104490491A CN 201110449049 A CN201110449049 A CN 201110449049A CN 102820476 A CN102820476 A CN 102820476A
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exchange membrane
proton exchange
battery
membrane
liquid phase
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CN102820476B (en
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马志啟
孙瑞玉
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/20—Manufacture of shaped structures of ion-exchange resins
    • C08J5/22—Films, membranes or diaphragms
    • C08J5/2206—Films, membranes or diaphragms based on organic and/or inorganic macromolecular compounds
    • C08J5/2218—Synthetic macromolecular compounds
    • C08J5/2256—Synthetic macromolecular compounds based on macromolecular compounds obtained by reactions other than those involving carbon-to-carbon bonds, e.g. obtained by polycondensation
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/497—Ionic conductivity
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
    • H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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Abstract

The invention relates to an application of a proton exchange membrane in an Fe-Cr system liquid phase fluid battery, and belongs to the liquid phase fluid battery application field. The proton exchange membrane has a selective permeability to hydrogen ions, the permeability of the proton exchange membrane to Fe<3+> at normal temperature and 65DEG C is 1200ug Fe<3+>/hr.cm<2>.M or less and 2500ug Fe<3+>/hr.cm<2>.M or less, and simultaneously the conductivity of the proton exchange membrane to an electrolyte solution at normal temperature under normal pressure is 0.03S.cm<-1> or more, or the resistivity of the membrane having a thickness of 120mum is 0.65 and 0.32omega.cm<2> or less. The proton exchange membrane is a sulfonated polyetheretherketone material anion exchange membrane or a sulfonated polyethersulfoneketone anion exchange membrane. According to the invention, a novel proton exchange membrane applied to fuel batteries at present is utilized as an isolation membrane, has a high-molecular membrane material based on hydrocarbons, and has a lower cost than perfluorosulfonic acid membranes. Compared with early-stage proton exchange membranes, the proton exchange membrane disclosed in the invention has the advantages of good proton selectivity, good conductivity, and maintenance of high efficiency and low cost of the battery.

Description

A kind of PEM is the application in the liquid phase fluid battery at iron-chromium
Technical field
The present invention relates to a kind of PEM is the application in the liquid phase fluid battery at iron-chromium.
Background technology
The liquid phase fluid energy-storage battery is a kind of energy conversion device, can be in electrolyte solution during charging with electrical power storage, and can former energy stored be transformed telegram in reply again during discharge can discharge.As its name suggests, its electrolyte solution is liquid condition, can electrolyte solution be sent to as required with delivery pump to carry out Conversion of energy in the battery or be sent in the storage tank preserving.Electrolyte solution storage tank, liquid circulation pump and external power source and load bearing chain connected components are the visual plant in the power-supply system.And battery is the nucleus equipment of whole accumulation power supply system.The characteristics determined of this kind battery its gather around and have broad application prospects, not only can be the key equipment and wind energy, solar association use in the intelligent grid in the future, also be the effective energy storage device that can serve traditional electrical network.
The battery pile that common liquid flow energy storage battery is stacked up and formed by a plurality of monocells.Battery pile can constitute more massive battery pile through the connection in series-parallel on electricity and (perhaps) fluid again, and its size depends on concrete Application Design.The structure of one of them monocell is made up of bipolar plates, positive electrode, electrolyte membrance (perhaps amberplex), negative electrode and bipolar plates.Wherein the core of battery system then is to be made up of positive electrode, negative electrode and the electrolyte membrance in the middle of them.Iron-chromium is that flow battery is a kind of of such liquid flow energy storage battery.Its work principle will be for containing Fe when beginning 2+Solution (like FeCl 2) be input on the anode in its storage tank by pump, will contain Cr 3+Solution (like CrCl 3) in its storage tank, be input on the GND.Electrolyte membrance between positive and negative electrode can be that the close film of matter also can be a perforated membrane, and it plays the effect of conduct charges carrier such as proton and other negative ions etc., and internal current is all through this barrier film when battery operated.Utilize external power source on two electrodes, to apply the voltage that is higher than battery equilibrium voltage (1.18V), just begin to have electrochemical reaction on the electrode, the charging beginning.Fe on the positive pole 2+Be converted to Fe 3+Cr on the while negative pole 3+Be converted to Cr 2+High-octane electrolyte solution after the conversion is cycled back in the storage tank separately and stores.Charging process is exactly to realize the conversion of chemical substance through the electrochemical reaction on the electrode, with the process of electrical power storage in electrolyte solution; Otherwise, externally during the need of load energy, the electrolyte solution in the storage tank being input in the battery via same method of fluid delivery, the outside has certain load to connect, and battery promptly begins discharge.Electrochemical reaction on the discharge process electrode is reverse carries out, and energy is discharged be sent to external loading.Under the condition of material settling out reasonable in design, system can realize the cycling that discharges and recharges again and again more frequently than traditional solid battery fully.
Therefore membrane materials for electrolyte plays crucial effects to the performance of battery.Iron-the chromium of taking as the leading factor with NASA (NASA) in early days is in the research of flow battery, is mostly the proton exchange membrane technology that adopts.Though and PEM conductivity has at that time satisfied the requirement of using, its selectivity is often undesirable, and with high costs.Conductivity and selectivity are a pair of implacable contradiction.Certainly its conductivity value mainly also depends on the concentration of acid in the electrolyte solution.Acid concentration is high, and conductivity is just high, but corrosivity is strong.The height of acid concentration also has very big influence to the concentration of effective ergastic substances in the electrolyte solution.Iron-chromium that present some company or mechanism are are researching and developing is that the flow battery product does not re-use the close PEM of matter in order to reduce cost, but replaces with cheap perforated membrane, does not have any ion selectivity.Though efficient still can reach more than 70%,, caused very big energy loss because inside battery is serious through the two poles of the earth electrolyte solution mixing phenomena of perforated membrane.
Summary of the invention
To defective and weak point that above-mentioned prior art exists, it is the application in the liquid phase fluid battery as the electrolyte barrier film at iron-chromium that the present invention provides a kind of novel proton exchange membranes that is applied to fuel cell at present.
The objective of the invention is to realize like this: a kind of PEM is the application in the liquid phase fluid battery at iron-chromium, and characteristics are that this PEM has the selection permeability for hydrogen ion, and it is to Fe 3+The permeability of ion is not higher than 1200 and 2500 μ g Fe respectively under normal temperature and 65 ℃ 3+/ hrcm 2M, its conductance is not less than 0.03Scm at normal temperatures and pressures for electrolyte solution simultaneously -1, the resistivity of the film that perhaps 120 μ m are thick is not more than 0.65 and 0.32 Ω cm 2
Said PEM preferred sulfonated polyether-ether-ketone material anion-exchange membrane or sulfonated polyether sulfone ketone material anion-exchange membrane.
Said PEM, film thickness are preferably between 20～300 μ m.
Said liquid phase fluid battery can be a monocell, or the battery pile of being made up of a plurality of batteries.
The structure of a monocell is made up of positive electrode, negative electrode and the PEM in the middle of them among the present invention; Positive electrode and negative electrode material are cavernous graphite carbon felt; Electrolyte solution can pass through the graphite carbon felt electrode; And electrochemical reaction takes place on electrode, accomplish the circulation of energy storage and exoergic.The operating voltage of monocell is usually between 0.6～1.2V.The present invention is the PEM that adopts, and it is selective to hydrogen ion, and only possibly have very small amount of seeing through to other cation, has good selectivity.In the research in early days, the cationic membrane of use that is PEM, it can pass through proton; Also through other metal cation; Selection permeability and conductance to proton are a pair of contradiction, and performance is undesirable, have caused the loss of certain internal current and stored energy capacitance.
The many forms with battery pile of flow battery occur, and exactly a plurality of monocells are stacked up, and realize the higher voltage range that is easy to use.Battery pile generally has general fluid passage, and the collection of considering electric current simultaneously is the two ends in battery pile, is to combine through bipolar plates between the monocell.Battery pile is made up of a plurality of monocells, and two ends are to be that positive electrode end plate, negative electrode end plate are fixed by two end plates, except two monocells at two ends, and public bipolar plates between the middle monocell.Simultaneously, share the fluid passage between all monocells.The design of integrated form can improve the energy density of battery and operation easily.Such battery pile structure makes Seal Design simple and reliable simultaneously, can realize that also battery pile is in the operation that needs under the operation with high pressure situation.
The present invention utilizes the novel proton exchange membranes that is applied to fuel cell at present as barrier film, and with respect to the sulfonate film of perfluor, this membrane material is based on the macromolecule member material of hydrocarbon, and relative cost is cheap.Compare with early stage PEM, it has good proton selectivity and conductivity.Make battery design not only keep higher efficient but also realized low cost.
Description of drawings:
Fig. 1 is a monocell internal structure sketch map of the present invention.
Fig. 2 is a battery pile structure sketch map of the present invention.
Embodiment:
Below in conjunction with specific embodiment the present invention is made further detailed description.
Embodiment 1:
Proton exchange membrane material is selected sulfonated polyether sulfone ketone (sPPESK) material PEM for use, and this membrane material is by RAI, and Inc. provides.Its preparation process summary is: the first step, and the polyethersulfone ketone powder is put into the agitated reactor adding concentrated sulfuric acid carry out sulfonation under certain conditions; In second step,, pour into film on the glass plate like routine through suitable film-forming process.
Present embodiment is applied to the Fe-Cr HTS flow battery with the membrane material sPPESK of above preparation.The internal structure of this Fe-Cr HTS flow battery monocell is as shown in Figure 1, is made up of positive electrode 2, negative electrode 3 and the PEM 1 in the middle of them.The version of battery pile is as shown in Figure 2, exactly a plurality of monocells stacked up, and be to combine between the monocell through bipolar plates.Two ends are to be that positive electrode end plate 4, negative electrode end plate 6 is fixing by two end plates, except two monocells at two ends, and public bipolar plates 5 between the middle monocell.
Concrete implementation process is: shear out the membrane material that a slice area is 7.5cm * 7.5cm, wherein effective area is 5cm * 4cm, and all the other areas are that sealing area contacts with sealing gasket.All have one of one of EPDM rubber gasket and the thick graphite carbon felt of 3mm to constitute positive and negative electrode in the both sides of film, the sealing gasket central part is cubic hole, and graphite carbon felt is arranged in cubic hole, also directly contacts with membrane material.In graphite carbon felt and the sealing gasket outside one of bipolar plates is arranged respectively, through bipolar plates and use suitable fasteners that all stratified materials are fixed together, promptly form a monocell.On every side bipolar plates liquid entrance is arranged all.Present embodiment only carries out the test of monocell, and the composition of battery pile is with reference to aforesaid way.Electrolytic liquid is to be transported in the battery through feed pump, and comes accurately to regulate the flow of liquid through certain control device.Heating is heating member to be set, the temperature of being regulated setting by temperature controller in fluid reservoir.The charging of battery, discharge are carried out according to certain procedure by DC power supply able to programme and DC electronic load respectively.
(Lewis Research Center, the comparative result of cationic membrane NASA) (code name is W285-99, and thickness 7mil does not have detailed material information) is seen table 1 for the performance of above-mentioned membrane material and notional result and Louis research institute of NASA.The sPPESK film that provides in the table is the close film of matter, only sees through proton in theory, has high selectivity.And the thickness of the film that can prepare is about 70micron, and at room temperature its resistivity has only 0.24 Ω cm 2, be about 1/5 of NASA film.When temperature was elevated to 65 ℃, its resistivity also can significantly descend.The performance of visible film under different temperatures in the table.Therefore the inside battery loss of voltage that utilizes this film all will be less than the battery of NASA, and the electrolyte solution between the both positive and negative polarity mixes less.So the complex energy conversion efficiency of its battery will be significantly increased, greater than 88%.
In addition, provide the influence of different film thicknesses to battery performance in the table, film thickness increases, and mechanical performance and better useful life preferably can be arranged, but the voltage drop meeting on the film increases to some extent, thereby voltage efficiency descends.Otherwise then voltage efficiency slightly rises, but enclosed pasture efficient may slightly descend, and the influence of comprehensive energy efficiency is little, all maintains higher level, all is superior to the performance of the early stage battery of delivering of NASA.
Embodiment 2:
Proton exchange membrane material is selected sulfonated polyether-ether-ketone material (sPEEK) PEM for use, and this membrane material is by RAI, and Inc. provides.Except polymerization macromolecule raw material polyether-ether-ketone was different with the raw material polyethersulfone ketone among the embodiment 1, the method and the film-forming method of membrane material sulfonation were similar, obtain the sPEEK film at last, and adopted identical battery tester.
(Lewis Research Center, the comparative result of cationic membrane NASA) is seen table 2 for the test performance of sPEEK film and notional result and Louis research institute of NASA.The sPEEK film that provides in the table also is the close film of matter, and is similar with the membrane material in the instance 1, only sees through proton in theory, has high selectivity.But at room temperature the film resistance rate of 70micron is omited height a bit, is 0.38 Ω cm 2, also be about NASA with 1/3 of film.When temperature was elevated to 65 ℃, its resistivity also can descend to some extent.Therefore the inside battery loss of voltage that utilizes this film all will be less than the battery of NASA, and the electrolyte solution between the both positive and negative polarity mixes less.So the complex energy conversion efficiency of its battery can reach more than 87%.
The comparison of table 1sPPESK film and NASA film
Figure BSA00000646191700051
* at 65C and optimum current density 60mA/cm 2
* 65 ℃ with normal pressure under, selectivity and energy efficiency are theoretical guess value
* * measured value at room temperature
The comparison of table 2sPEEK film and NASA film
Figure BSA00000646191700052
* at 65 ℃ and optimum current density 60mA/cm 2
* 65 ℃ with normal pressure under, selectivity and energy efficiency are theoretical guess value
* * measured value at room temperature

Claims (5)

1. a PEM is the application in the liquid phase fluid battery at iron-chromium, it is characterized in that this PEM has the selection permeability for hydrogen ion, and it is to Fe 3+The permeability of ion is not higher than 1200 and 2500 μ g Fe respectively under normal temperature and 65 ℃ 3+/ hrcm 2M, its conductance is not less than 0.03Scm at normal temperatures and pressures for electrolyte solution simultaneously -1, the resistivity of the film that perhaps 120 μ m are thick is not more than 0.65 and 0.32 Ω cm 2
2. application according to claim 1 is characterized in that said PEM is a sulfonated polyether-ether-ketone material anion-exchange membrane.
3. application according to claim 1 is characterized in that said PEM is a sulfonated polyether sulfone ketone material anion-exchange membrane.
4. according to claim 1 or 2 or 3 described application, it is characterized in that said PEM, film thickness is between 20～300 μ m.
5. according to claim 1 or 2 or 3 described application, it is characterized in that said liquid phase fluid battery is a monocell, or the battery pile of forming by a plurality of batteries.
CN201110449049.1A 2011-12-29 2011-12-29 The application of a kind of proton exchange membrane in iron-chromium system liquid phase fluid battery Expired - Fee Related CN102820476B (en)

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PCT/CN2012/086301 WO2013097595A1 (en) 2011-12-29 2012-12-10 Use of proton exchange membrane in iron-chromium liquid fluid battery
EP12863711.3A EP2800181A4 (en) 2011-12-29 2012-12-10 Use of proton exchange membrane in iron-chromium liquid fluid battery

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CN108511778A (en) * 2018-03-15 2018-09-07 上海晶璇企业管理咨询有限公司 A kind of iron-chrome liquor galvanic battery and electrolyte solution and dosing apparatus and preparation method
CN109065925A (en) * 2018-07-23 2018-12-21 中国科学院金属研究所 A kind of Iron/chromium Redox Flow Cell non-fluorine both sexes composite membrane and preparation method
TWI796024B (en) * 2021-11-30 2023-03-11 財團法人金屬工業研究發展中心 Fluid battery module

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Cited By (5)

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Publication number Priority date Publication date Assignee Title
CN108511778A (en) * 2018-03-15 2018-09-07 上海晶璇企业管理咨询有限公司 A kind of iron-chrome liquor galvanic battery and electrolyte solution and dosing apparatus and preparation method
CN108511778B (en) * 2018-03-15 2021-05-14 上海晶璇企业管理咨询有限公司 Iron-chromium flow battery, electrolyte solution, preparation equipment and preparation method
CN109065925A (en) * 2018-07-23 2018-12-21 中国科学院金属研究所 A kind of Iron/chromium Redox Flow Cell non-fluorine both sexes composite membrane and preparation method
CN109065925B (en) * 2018-07-23 2021-07-23 中国科学院金属研究所 Non-fluorine amphoteric composite membrane for iron-chromium redox flow battery and preparation method
TWI796024B (en) * 2021-11-30 2023-03-11 財團法人金屬工業研究發展中心 Fluid battery module

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